High Piezoelectric Performance in Pb(Ni_1/3Nb_2/3)O₃–Pb(Sc_1/2Nb_1/2)O₃–PbTiO₃ Ternary System Featuring Small Structural Distortion and Heterogeneous Domain Configuration

Abstract

Ternary/polynary perovskite solid solutions based on binary systems are well-known for their high piezoelectric performance. In this work, a series of Pb(Ni 1/3 Nb 2/3 )O 3 − Pb(Sc 1/2 Nb 1/2 )O 3 −PbTiO 3 compositions with the particularly high piezoelectric coefficient of d 33 * > 1000 pm/V and d 33 > 700 pC/N have been developed. The optimal performance was achieved in the 0.52PNN-0.14PSN-0.34PT composition (d 33 * = 1120 pm/V, d 33 = 804 pC/N, and T m = 109 °C). The high piezoelectric performance of this system is reported and is superior to those of most lead-based ternary/polynary ceramics. By a combination of in situ high-energy synchrotron diffraction with transmission electron microscopy (TEM), the origin of the high piezoelectric response has been unambiguously revealed. Upon application of an external electric field, synchrotron diffraction profiles show no splitting but prominent shifting, indicating that the large intrinsic lattice strain arising from the reduced crystal anisotropy and facilitated polarization variation is associated with the high piezoelectric response. Furthermore, microscopic studies by TEM highlight a heterogeneous ferroelectric domain configuration generated by a small local structural distortion, which is also beneficial for the high piezoelectric performance in the proposed ternary piezoelectric systems. The design process of ternary perovskite solid solutions with a wide morphotropic phase boundary region and small structural distortion may be enlightening for the exploration of other high-performance polynary piezoelectrics.

High‐performance ferroelectric based materials via high‐entropy strategy: Design, properties, and mechanism

“…Recently, a high-entropy strategy to design high piezoelectricity was proposed by introducing ions with different radius and valence states into B-site to regulate polarization configuration, and a series of lead-based systems with outstanding performance of d 33 > 800 pC N À1 was successfully obtained in Pb-based piezoceramics. [63][64][65] With gradually adding B-site elements, an ultrahigh d 33 of $1200 pC N À1 was achieved in a Pb(Ni 0.173 In 0.07 Zr 0.034 Ti 0.306 Nb 0.417 )O 3 composition with five different elements sharing one lattice position (Figure 7A). Meanwhile, the piezoelectric coefficient is strongly correlated with configuration entropy, which proves that the high-entropy strategy is reliable in realizing high piezoelectric performance because of the enhanced disorder degree of B-site (Figure 7B).…”

“…According to the above introduction, it can be found the increased polarization configurational disorder in FEs has been proven to be beneficial for performance improvement, which can be directly realized by the high‐entropy strategy. Recently, a high‐entropy strategy to design high piezoelectricity was proposed by introducing ions with different radius and valence states into B‐site to regulate polarization configuration, and a series of lead‐based systems with outstanding performance of d 33 > 800 pC N −1 was successfully obtained in Pb‐based piezoceramics 63–65 . With gradually adding B‐site elements, an ultrahigh d 33 of ~1200 pC N −1 was achieved in a Pb(Ni 0.173 In 0.07 Zr 0.034 Ti 0.306 Nb 0.417 )O 3 composition with five different elements sharing one lattice position (Figure 7A).…”

“…Beyond piezoelectricity, 60,63–66 considerable strides have also been made in ferroelectricity, 53,59,67 relaxor FE behavior, 61 dielectric permittivity and loss, 68,69 and dielectric relaxation 70 in FEs engineering by elevating configuration entropy. For instance, an A‐site equimolar (Pb 0.25 Ba 0.25 Sr 0.25 Ca 0.25 )TiO 3 medium‐entropy relaxor FE system boasting a configuration entropy of 1.39 R demonstrated low loss (<0.015).…”

A synergistic approach to attain high piezoelectricity in a Pb(Ni, Nb)O3–Pb(Lu, Nb)O3–PbTiO3 system

“…21,22 Based on MPB engineering, researchers have developed numerous multiphase ceramics with excellent properties. [23][24][25][26][27] For example, multiphase coexistence is designed in the Pb(Ni, Nb)O 3 -Pb(Hf, Ti)O 3 23 (PNN-PHT) and Pb(Ni, Nb)O 3 -Pb(Sc, thermodynamic energy profile to improve piezoelectricity, such as introducing a local heterostructure and resulting generation of polar nanoregions (PNRs) by the short-range ordering of B-site cations at the nanoscale or aliovalent doping of the A-site, which could smooth the free energy barrier to promote polarization rotation when stimulated by an external electric field. 17,28 Moreover, the competition between Landau energy and interfacial energies can flatten the free energy distribution and increase the piezoelectric response.…”

“…21,22 Based on MPB engineering, researchers have developed numerous multiphase ceramics with excellent properties. 23–27 For example, multiphase coexistence is designed in the Pb(Ni, Nb)O 3 –Pb(Hf, Ti)O 3 23 (PNN–PHT) and Pb(Ni, Nb)O 3 –Pb(Sc, Nb)O 3 –PbTiO 3 25 (PNN–PSN–PT) systems, resulting in an ultrahigh piezoelectric response ( d 33 = 970 pC N −1 and 804 pC N −1 ).…”